{"title":"重新评估CH3NH3PbI3钙钛矿薄膜中电流/电压和稳态光载流子光栅测量值的解释","authors":"M. Córdoba , M. Berruet , K. Taretto","doi":"10.1016/j.jpcs.2025.112961","DOIUrl":null,"url":null,"abstract":"<div><div>The temperature dependence of optoelectronic parameters in halide perovskites is challenging to access due to the interplay between ionic migration, electronic transport, and structural phase transitions. This study combines current/voltage <em>J(V)</em> characteristics and steady-state photocarrier grating (SSPG) measurements, integrating classical and perovskite-specific physics. The forward <em>J(V)</em> curves reveal a transition from a sub–Ohmic regime to higher-order regimes, governed by ion dynamics. Assuming that grain boundaries hinder ion diffusion, the time and temperature required for this transition provide critical material parameters. In solution-prepared MAPI films, we determine an activation energy of 0.43 eV for the apparent dielectric constant and a room-temperature ion diffusion coefficient of 1.4 × 10<sup>−11</sup> cm<sup>2</sup>/s with an activation energy of 0.48 eV, consistent with published values obtained by more sophisticated methods. Under illumination, <em>J(V)</em> curves show increased photoconductivity with temperature, with activation energies between 0.12 and 0.25 eV, explained by recombination dominated by shallow defects. SSPG measurements indicate ambipolar diffusion lengths of 100–200 nm at room temperature, increasing tenfold at 65 °C, i.e. in the cubic phase. This increase is attributed to a rise in dielectric relaxation time above the tetragonal-to-cubic phase transition at 40 °C, rather than enhanced carrier lifetimes, providing new insights into perovskite characterization.</div></div>","PeriodicalId":16811,"journal":{"name":"Journal of Physics and Chemistry of Solids","volume":"207 ","pages":"Article 112961"},"PeriodicalIF":4.3000,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Reassessing the interpretation of current/voltage and steady–state photocarrier grating measurements in CH3NH3PbI3 perovskite films across device-operation temperatures\",\"authors\":\"M. Córdoba , M. Berruet , K. Taretto\",\"doi\":\"10.1016/j.jpcs.2025.112961\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The temperature dependence of optoelectronic parameters in halide perovskites is challenging to access due to the interplay between ionic migration, electronic transport, and structural phase transitions. This study combines current/voltage <em>J(V)</em> characteristics and steady-state photocarrier grating (SSPG) measurements, integrating classical and perovskite-specific physics. The forward <em>J(V)</em> curves reveal a transition from a sub–Ohmic regime to higher-order regimes, governed by ion dynamics. Assuming that grain boundaries hinder ion diffusion, the time and temperature required for this transition provide critical material parameters. In solution-prepared MAPI films, we determine an activation energy of 0.43 eV for the apparent dielectric constant and a room-temperature ion diffusion coefficient of 1.4 × 10<sup>−11</sup> cm<sup>2</sup>/s with an activation energy of 0.48 eV, consistent with published values obtained by more sophisticated methods. Under illumination, <em>J(V)</em> curves show increased photoconductivity with temperature, with activation energies between 0.12 and 0.25 eV, explained by recombination dominated by shallow defects. SSPG measurements indicate ambipolar diffusion lengths of 100–200 nm at room temperature, increasing tenfold at 65 °C, i.e. in the cubic phase. This increase is attributed to a rise in dielectric relaxation time above the tetragonal-to-cubic phase transition at 40 °C, rather than enhanced carrier lifetimes, providing new insights into perovskite characterization.</div></div>\",\"PeriodicalId\":16811,\"journal\":{\"name\":\"Journal of Physics and Chemistry of Solids\",\"volume\":\"207 \",\"pages\":\"Article 112961\"},\"PeriodicalIF\":4.3000,\"publicationDate\":\"2025-06-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Physics and Chemistry of Solids\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0022369725004135\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Physics and Chemistry of Solids","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0022369725004135","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Reassessing the interpretation of current/voltage and steady–state photocarrier grating measurements in CH3NH3PbI3 perovskite films across device-operation temperatures
The temperature dependence of optoelectronic parameters in halide perovskites is challenging to access due to the interplay between ionic migration, electronic transport, and structural phase transitions. This study combines current/voltage J(V) characteristics and steady-state photocarrier grating (SSPG) measurements, integrating classical and perovskite-specific physics. The forward J(V) curves reveal a transition from a sub–Ohmic regime to higher-order regimes, governed by ion dynamics. Assuming that grain boundaries hinder ion diffusion, the time and temperature required for this transition provide critical material parameters. In solution-prepared MAPI films, we determine an activation energy of 0.43 eV for the apparent dielectric constant and a room-temperature ion diffusion coefficient of 1.4 × 10−11 cm2/s with an activation energy of 0.48 eV, consistent with published values obtained by more sophisticated methods. Under illumination, J(V) curves show increased photoconductivity with temperature, with activation energies between 0.12 and 0.25 eV, explained by recombination dominated by shallow defects. SSPG measurements indicate ambipolar diffusion lengths of 100–200 nm at room temperature, increasing tenfold at 65 °C, i.e. in the cubic phase. This increase is attributed to a rise in dielectric relaxation time above the tetragonal-to-cubic phase transition at 40 °C, rather than enhanced carrier lifetimes, providing new insights into perovskite characterization.
期刊介绍:
The Journal of Physics and Chemistry of Solids is a well-established international medium for publication of archival research in condensed matter and materials sciences. Areas of interest broadly include experimental and theoretical research on electronic, magnetic, spectroscopic and structural properties as well as the statistical mechanics and thermodynamics of materials. The focus is on gaining physical and chemical insight into the properties and potential applications of condensed matter systems.
Within the broad scope of the journal, beyond regular contributions, the editors have identified submissions in the following areas of physics and chemistry of solids to be of special current interest to the journal:
Low-dimensional systems
Exotic states of quantum electron matter including topological phases
Energy conversion and storage
Interfaces, nanoparticles and catalysts.